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Boosting Solid-State Diffusivity and Conductivity in Lithium Superionic Argyrodites by Halide Substitution.

Parvin Adeli1, J David Bazak2, Kern Ho Park1

  • 1Department of Chemistry and the Waterloo Institute for Nanotechnology, University of Waterloo, Waterloo, Ontario, N2L 3G1, Canada.

Angewandte Chemie (International Ed. in English)
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PubMed
Summary
This summary is machine-generated.

New solid electrolyte phases in the Li6 PS5 Cl family show enhanced lithium-ion conductivity. Increasing the chloride content significantly boosts ionic diffusivity for advanced all-solid-state batteries.

Keywords:
Li-ion conductorPFG NMR spectroscopyargyroditeneutron diffractionsolid electrolyte

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Solid-State Chemistry

Background:

  • High-performance all-solid-state batteries require solid electrolytes with high ionic conductivity and ductility.
  • The argyrodite Li6 PS5 Cl family is a promising class of solid electrolytes.
  • Understanding structure-property relationships is crucial for optimizing ionic transport.

Purpose of the Study:

  • To investigate new halide-rich solid solution phases within the Li6 PS5 Cl family.
  • To determine the impact of varying chloride (Cl-) to sulfide (S2-) ratios on lithium-ion (Li+) diffusivity.
  • To correlate structural changes with enhanced ionic conductivity.

Main Methods:

  • Synthesis of Li6-x PS5-x Cl1+x solid solution phases.
  • Electrochemical impedance spectroscopy to measure ionic conductivity.
  • Neutron diffraction and 7 Li Nuclear Magnetic Resonance (NMR) MAS and PFG spectroscopy for structural and diffusion analysis.

Main Results:

  • A systematic increase in Li+ -ion diffusivity was observed with increasing Cl- /S2- ratio.
  • The phase Li5.5 PS4.5 Cl1.5 achieved a cold-pressed conductivity of 9.4 mS cm-1 at 298 K, nearly four times higher than Li6 PS5 Cl.
  • Enhanced Li+ -ion transport is attributed to weakened Li+ -anion interactions, increased site disorder, and higher lithium vacancy concentrations.

Conclusions:

  • Substitution of S2- with Cl- in the Li6 PS5 Cl argyrodite structure significantly enhances ionic conductivity.
  • The halide-rich solid solution phases offer a viable pathway to developing advanced solid electrolytes for all-solid-state batteries.
  • These findings provide critical insights into designing solid electrolytes with superior electrochemical performance.